Dr Stefano Leoni
Darllenydd mewn Cemeg Gyfrifiadurol
- Ar gael fel goruchwyliwr ôl-raddedig
Trosolwyg
Links
Research Groups: Inorganic Chemistry
Research Interests
The Leoni group focuses on the study of activated processes in the solid state by means of advanced computational tools. Structural and electronic phase transitions, chemical reactions, formation mechanisms, reactive intermediates, structure prediction and the rules behind polymorphism in general are relevant research areas. Understanding processes like crystallization, nucleation and growth, diffusion of impurities or defects, or electrochemical reactions are crucial factors for the development of better materials. Despite major advances in device resolution, experiments can only provide a coarse-grained view of such processes. Theory can now integrate the experimental data by implementing the missing length and time resolution, thanks to novel strategies of numerical simulations. At the interface of inorganic and material sciences, theoretical chemistry, computational chemistry and physics, physical chemistry, materials for energy and sustainability, this area offers fascinating opportunities to leverage computational tools in the design of innovative materials.
Cyhoeddiad
2024
- Sheng, Y. et al. 2024. Confinement and synergy effects of supported-confined bimetal catalysts with superior stability and catalytic activity. Journal of Energy Chemistry 99, pp. 93-99. (10.1016/j.jechem.2024.07.022)
- Al Zoubi, W., Leoni, S., Assfour, B., Allaf, A. W., Kang, J. and Ko, Y. G. 2024. Continuous synthesis of metal oxide‐supported high‐entropy alloy nanoparticles with remarkable durability and catalytic activity in the hydrogen reduction reaction. InfoMat (10.1002/inf2.12617)
- Flack, T., Jobbins, S. A., Boulfelfel, S. E. and Leoni, S. 2024. Many-Particle Na-Ion Dynamics in NaMPO4 Olivine Phosphates (M = Mn, Fe). In: Hanaor, D. A. H. ed. Computational Design of Battery Materials., Vol. 150. Springer, Cham, pp. 137-167., (10.1007/978-3-031-47303-6_5)
- Al Zoubi, W., Al Mahmud, A., Hazmatulhaq, F., Thalji, M. R., Leoni, S., Kang, J. and Ko, Y. G. 2024. Origin of the synergistic effects of bimetallic nanoparticles coupled with a metal oxide heterostructure for accelerating catalytic performance. SusMat 4(3), article number: e216. (10.1002/sus2.216)
- Craco, L. and Leoni, S. 2024. Strange metal and coherence-incoherence crossover in pressurized La3Ni2O7. Physical Review B (Condensed Matter and Materials Physics) 109(16), article number: 165116. (10.1103/PhysRevB.109.165116)
- Craco, L. and Leoni, S. 2024. Effect of localization–delocalization transition on thermoelectric properties of Bi2Te2Se topological insulator. APL Energy 2(1), article number: 16102. (10.1063/5.0173308)
2023
- Craco, L. and Leoni, S. 2023. Normal-state correlated electronic structure of the tetragonal TlNi2Se2 superconductor. Physical Review B 108(4), article number: 45140. (10.1103/PhysRevB.108.045140)
- Craco, L. and Leoni, S. 2023. Orbital-selective mixed-valent Mott/metal phase coexistence in NdNiO2 films. Physical Review Materials 7(4), article number: 44802. (10.1103/PhysRevMaterials.7.044802)
- Al Zoubi, W., Assfour, B., Wahab Allaf, A., Leoni, S., Kang, J. and Ko, Y. G. 2023. Experimental and theoretical investigation of high-entropy-alloy/support as a catalyst for reduction reactions.. Journal of Energy Chemistry 81, pp. 132-142. (10.1016/j.jechem.2023.02.042)
2022
- Craco, L., de Arruda, A. S. and Leoni, S. 2022. Emergent normal-state Mottness in the infinite-layer NdNiO 2 superconductor. Physical Review Research 4(4), article number: 43036. (10.1103/PhysRevResearch.4.043036)
- Kaußler, C. et al. 2022. "Dynamical docking" of cyclic dinuclear au(i) bis-n-heterocyclic complexes facilitates their binding to g-quadruplexes. Inorganic Chemistry 61(50), article number: 20405. (10.1021/acs.inorgchem.2c03041)
- Selli, D., Baburin, I. A., Martonák, R. and Leoni, S. 2022. Ge136 type-II clathrate as precursor for the synthesis of metastable germanium polymorphs: a computational study. Physical Review B 106(17), article number: 174102. (10.1103/PhysRevB.106.174102)
- Osypiw, A. et al. 2022. Solution-processed colloidal quantum dots for light emission. Materials Advances 3, pp. 6773-6790. (10.1039/D2MA00375A)
- Rundle, J. and Leoni, S. 2022. Layered tin chalcogenides SnS and SnSe: lattice thermal conductivity benchmarks and thermoelectric figure of merit. Journal of Physical Chemistry C 126(33), pp. 14036–14046. (10.1021/acs.jpcc.2c02401)
- Selli, D., Donadio, D. and Leoni, S. 2022. PbTe/PbSe thermoelectric nanocomposites: the impact of length modulations on lowering thermal conductivity. Journal of Inorganic and General Chemistry 648(15), article number: e202200048. (10.1002/zaac.202200048)
- Flack, T., Jobbins, S. A., Boulfelfel, S. E. and Leoni, S. 2022. Many-particle Li Ion dynamics in LiMPO4 olivine phosphates (M = Mn, Fe). Journal of Physical Chemistry C 126(30), pp. 12339-12347. (10.1021/acs.jpcc.2c02013)
- Ryník, M., Leoni, S. and Martonák, R. 2022. Pressure-induced structural transformation of clathrate Ge136 via ultrafast recrystallization of an amorphous intermediate. Physical Review B 105(13), article number: 134107. (10.1103/PhysRevB.105.134107)
- Craco, L. and Leoni, S. 2022. Orbital selectivity in the normal state of KFe(2)Se(2) superconductor. European Physical Society Letters 136(2), article number: 27002. (10.1209/0295-5075/ac3f16)
2021
- Pimpao, C. et al. 2021. Mechanisms of irreversible aquaporin-10 inhibition by organogold compounds studied by combined biophysical methods and atomistic simulations. Metallomics 13(9), article number: mfab053. (10.1093/mtomcs/mfab053)
- Craco, L., Carara, S. S. and Leoni, S. 2021. Landau-Fermi liquidness and s-wave superconducting properties of pressurized gray phosphorus. The European Physical Journal B 94(5), article number: 115. (10.1140/epjb/s10051-021-00121-y)
- Craco, L. and Leoni, S. 2021. Orbital-selective nature of the 3d electronic structure of the ThFeAsN superconductor. Physical Review B 103(7), article number: 75110. (10.1103/PhysRevB.103.075110)
- Craco, L., Carara, S. S. and Leoni, S. 2021. Interplay of electric field and disorder in Dirac liquid silicene. The European Physical Journal B 94(2), article number: 47. (10.1140/epjb/s10051-021-00055-5)
2020
- Wragg, D., Leoni, S. and Casini, A. 2020. Aquaporin-driven hydrogen peroxide transport: a case of molecular mimicry?. RSC Chemical Biology 1(5), pp. 390-394. (10.1039/D0CB00160K)
- Craco, L. and Leoni, S. 2020. All-t2g electronic orbital reconstruction of monoclinic MoO2 battery material. Applied Sciences 10(17), article number: 5730. (10.3390/app10175730)
- Craco, L. and Leoni, S. 2020. Mott and pseudogap localization in pressurized NbO2. Physical Review B 102(4), article number: 45142. (10.1103/PhysRevB.102.045142)
- Craco, L. and Leoni, S. 2020. Pressure-induced orbital-selective metal from the Mott insulator BaFe2Se3. Physical Review B 101(24), article number: 245133. (10.1103/PhysRevB.101.245133)
- Wragg, D., Casini, A. and Leoni, S. 2020. Harvesting free energy landscapes in biological systems. Presented at: International Conference on Bio and Nanomaterials, MSC Cruise, Mediterranean Sea, Italy, 28 Sept - 3 Oct 2019 Presented at Piotto, S. et al. eds.Advances in Bionanomaterials II. Lecture Notes in Bioengineering Springer pp. 64-77., (10.1007/978-3-030-47705-9_7)
2019
- Craco, L. and Leoni, S. 2019. LDA+DMFT approach to electronic structure of sodium metal. Physical Review B 100(11), article number: 115156. (10.1103/PhysRevB.100.115156)
- Craco, L. and Leoni, S. 2019. Theory of two-fluid metallicity in superconducting FeSe at high pressure. Physical Review B 100(12), pp. -., article number: 121101. (10.1103/PhysRevB.100.121101)
- Wragg, D., de Almeida, A., Casini, A. and Leoni, S. 2019. Unveiling the mechanisms of aquaglyceroporin-3 water and glycerol permeation by metadynamics. Chemistry - A European Journal 25(37), pp. 8713-8718. (10.1002/chem.201902121)
- Craco, L., Carara, S. S. and Leoni, S. 2019. Electronic structure of BiFeO3 in the presence of strong electronic correlations. Physical Review B 99(4), pp. -., article number: 45112. (10.1103/PhysRevB.99.045112)
- Fang, H. et al. 2019. Structural tuning and catalysis of tungsten carbides for the regioselective cleavage of C-O bonds. Journal of Catalysis 369, pp. 283-295. (10.1016/j.jcat.2018.11.020)
2018
- Mósca, A. F. et al. 2018. Molecular basis of Aquaporin-7 permeability regulation by pH. Cells 7(11), article number: 207. (10.3390/cells7110207)
- Craco, L. and Leoni, S. 2018. Microscopic description of localization-delocalization transitions in BaFe2S3. Physical Review B 98(19), pp. -., article number: 195107. (10.1103/PhysRevB.98.195107)
- Wragg, D., De Almeida, A., Bonsignore, R., Kühn, F. E., Leoni, S. and Casini, A. 2018. On the mechanism of Gold/NHC compounds binding to DNA G-quadruplexes: combined metadynamics and biophysical methods. Angewandte Chemie International Edition 57(44), pp. 14524-14528. (10.1002/anie.201805727)
- Jobbins, S. A., Boulfelfel, S. E. and Leoni, S. 2018. Metashooting: a novel tool for free energy reconstruction from polymorphic phase transition mechanisms. Faraday Discussions 211, pp. 235-251. (10.1039/C8FD00053K)
- Rocard, L., Wragg, D., Jobbins, S. A., Luciani, L., Leoni, S., Wouters, J. and Bonifazi, D. 2018. Templated chromophore assembly on peptide scaffolds: a structural evolution. Chemistry - A European Journal, pp. -. (10.1002/chem.201803205)
- Craco, L., Freelon, B., Alafailakawi, A. M., Karki, B. and Leoni, S. 2018. Site-selective electronic structure of pure and doped Ca2 O3 Fe3 S2. Physical Review B 98(4), pp. -., article number: 45130. (10.1103/PhysRevB.98.045130)
- Craco, L., Pereira, T. A. d. S., Ferreira, S. R., Carara, S. S. and Leoni, S. 2018. Kondo-semimetal to Fermi-liquid phase crossover in black phosphorus to pressure-induced orbital-nematic gray phosphorus. Physical Review B 98(3), pp. -., article number: 35114. (10.1103/PhysRevB.98.035114)
- Paściak, M., Welberry, T. R., Kulda, J., Leoni, S. and Hlinka, J. 2018. Dynamic displacement disorder of cubic BaTiO3. Physical Review Letters 120(16), pp. -., article number: 167601. (10.1103/PhysRevLett.120.167601)
2017
- Craco, L., Pereira, T. A. d. S. and Leoni, S. 2017. Electronic structure and thermoelectric transport of black phosphorus. Physical Review B 96(7), article number: 75118. (10.1103/PhysRevB.96.075118)
- Craco, L., Laad, M. S. and Leoni, S. 2017. Microscopic description of insulator-metal transition in high-pressure oxygen. Scientific Reports 7, article number: 2632. (10.1038/s41598-017-02730-z)
- De Almeida, A. et al. 2017. The mechanism of aquaporin inhibition by gold compounds elucidated by biophysical and computational methods. Chemical Communications 53(27), pp. 3830-3833. (10.1039/C7CC00318H)
- Craco, L. and Leoni, S. 2017. Selective orbital reconstruction in tetragonal FeS: A density functional dynamical mean-field theory study. Scientific Reports 7, article number: 46439. (10.1038/srep46439)
- Craco, L., Faria, J. L. B. and Leoni, S. 2017. Electronic reconstruction of hexagonal FeS: a view from density functional dynamical mean-field theory. Materials Research Express 4(3), article number: 36303. (10.1088/2053-1591/aa6296)
- Springer, S., Heidenreich, N., Stock, N., van Wüllen, L., Huber, K., Leoni, S. and Wiebcke, M. 2017. The ZIF system zinc(II) 4,5-dichoroimidazolate: theoretical and experimental investigations of the polymorphism and crystallization mechanisms. Zeitschrift für Kristallographie - Crystalline Materials 232(1-3), pp. 77-90. (10.1515/zkri-2016-1968)
- Fang, H., Zheng, J., Luo, X., Du, J., Roldan Martinez, A., Leoni, S. and Yuan, Y. 2017. Product tunable behavior of carbon nanotubes-supported Ni?Fe catalysts for guaiacol hydrodeoxygenation. Applied Catalysis A: General 529, pp. 20-31. (10.1016/j.apcata.2016.10.011)
2016
- Craco, L., Carara, S. S. and Leoni, S. 2016. Band narrowing and Mott localization in isotropically superstrained graphene. Physical Review B 94(16), article number: 165168. (10.1103/PhysRevB.94.165168)
- Springer, S., Baburin, I., Heinemeyer, T., Gerrit Schiffmann, J., van Wullen, L., Leoni, S. and Wiebcke, M. 2016. A zeolitic imidazolate framework with conformational variety: Conformational polymorphs versus frameworks with static conformational disorder. Crystengcomm 18(14), pp. 2477-2489. (10.1039/C6CE00312E)
- Grundy, D. J., Chen, M., Gonzalez, V., Leoni, S., Miller, D. J., Christianson, D. W. and Allemann, R. K. 2016. Mechanism of germacradien-4-ol synthase controlled water capture. Biochemistry 55(14), pp. 2112-2121. (10.1021/acs.biochem.6b00115)
- Selli, D., Boulfelfel, S. E., Schapotschnikow, P., Donadio, D. and Leoni, S. 2016. Hierarchical thermoelectrics: crystal grain boundaries as scalable phonon scatterers. Nanoscale 8(6), pp. 3729-3728. (10.1039/C5NR05279C)
2015
- Freelon, B. et al. 2015. Mott-Kondo insulator behavior in the iron oxychalcogenides. Physical Review B 92(15), article number: 155139. (10.1103/PhysRevB.92.155139)
- Behrens, K. et al. 2015. Microwave-assisted synthesis of defects metal-imidazolate-amide-imidate frameworks and improved CO2 capture. Inorganic Chemistry 54(20), pp. 10073-10080. (10.1021/acs.inorgchem.5b01952)
- Craco, L., Selli, D., Seifert, G. and Leoni, S. 2015. Revealing the hidden correlated electronic structure of strained graphene. Physical Review B 91(20), article number: 205120. (10.1103/PhysRevB.91.205120)
- Craco, L. and Leoni, S. 2015. Magnetoresistance in the spin-orbit kondo state of elemental bismuth. Scientific Reports 5(1), pp. -., article number: 13772. (10.1038/srep13772)
2014
- Craco, L. and Leoni, S. 2014. Effect of band filling in the paramagnetic tetragonal phase of iron chalcogenides. Materials Research Express 1(3), article number: 36001. (10.1088/2053-1591/1/3/036001)
- Boulfelfel, S. E., Selli, D. and Leoni, S. 2014. Novel carbons: habits and oddities. Journal of Inorganic and General Chemistry 640(5), pp. 681-688. (10.1002/zaac.201300652)
- Schweinefuß, M. E., Springer, S., Baburin, I. A., Hikov, T., Huber, K., Leoni, S. and Wiebcke, M. 2014. Zeolitic imidazolate framework-71 nanocrystals and a novel SOD-type polymorph: solution mediated phase transformations, phase selection via coordination modulation and a density functional theory derived energy landscape. Dalton Transactions 43(9), pp. 3528-3536. (10.1039/c3dt52992d)
- Pasciak, M., Welberry, T., Heerdegen, A., Laguta, V., Ostapchuk, T., Leoni, S. and Hlinka, J. 2014. Atomistic modeling of diffuse scattering in cubic PbZrO3. Phase Transitions 88(3), pp. 273-28. (10.1080/01411594.2014.981266)
- Schröder, C. A., Saha, S., Huber, K., Leoni, S. and Wiebcke, M. 2014. Metastable metal imidazolates: development of targeted syntheses by combining experimental and theoretical investigations of the formation mechanisms. Zeitschrift fur Kristallographie Crystalline Materials 229(12), pp. 807-822. (10.1515/zkri-2014-1788)
- Craco, L., Laad, M. S. and Leoni, S. 2014. Orbital-selective mottness in layered iron oxychalcogenides: the case of Na2Fe2OSe2. Journal of Physics: Condensed Matter 26(14), pp. -., article number: 145602. (10.1088/0953-8984/26/14/145602)
- Craco, L., Laad, M. S. and Leoni, S. 2014. Normal-state correlated electronic structure of tetragonal FeSe superconductor. Journal of Physics: Conference Series 487, pp. -., article number: 12017. (10.1088/1742-6596/487/1/012017)
- Leoni, S., Boulfelfel, S. E., Baburin, I. A. and Selli, D. 2014. The rules of metastability: detailed transformation mechanisms in chemical elements by means of molecular dynamics techniques. In: Springborg, M. and Joswig, J. eds. Chemical Modelling : Volume 11., Vol. 11. Royal Society of Chemistry, pp. 30.
- Schweinefuß, M. E., Baburin, I. A., Schröder, C. A., Näther, C., Leoni, S. and Wiebcke, M. 2014. Indium imidazolate frameworks with differently distorted ReO3-type structures: syntheses, structures, phase transitions, and crystallization studies. Crystal Growth and Design 14(9), pp. 4664-4673. (10.1021/cg5007499)
2013
- Selli, D., Baburin, I. A., Martonák, R. and Leoni, S. 2013. Novel metastable metallic and semiconducting germaniums. Scientific Reports 3, article number: 1466. (10.1038/srep01466)
- Schröder, C. A., Baburin, I. A., van Wüllen, L., Wiebcke, M. and Leoni, S. 2013. Subtle polymorphism of zinc imidazolate frameworks: temperature-dependent ground states in the energy landscape revealed by experiment and theory. Crystengcomm 15(20), pp. 4036-4040. (10.1039/c2ce26045j)
- Baldoni, M., Craco, L., Seifert, G. and Leoni, S. 2013. A two-electron mechanism of lithium insertion into layered α-MoO3: a DFT and DFT+U study. Journal of Materials Chemistry A 1(5), pp. 1778-1784. (10.1039/c2ta00839d)
2012
- Debatin, F. et al. 2012. An isoreticular family of microporous metal-organic frameworks based on zinc and 2-substituted imidazolate-4-amide-5-imidate: syntheses, structures and properties. Chemistry - a European Journal 18(37), pp. 11630-11640. (10.1002/chem.201200889)
- Boulfelfel, S. E., Oganov, A. R. and Leoni, S. 2012. Understanding the nature of 'superhard graphite'. Scientific Reports 2, article number: 471. (10.1038/srep00471)
2011
- Assfour, B., Leoni, S., Seifert, G. and Baburin, I. A. 2011. Packings of carbon nanotubes - new materials for hydrogen storage. Advanced Materials 23(10), pp. 1237-1241. (10.1002/adma.201003669)
2008
- Leoni, S., Ramlau, R., Meier, K., Schmidt, M. and Schwarz, U. 2008. Nanodomain fragmentation and local rearrangements in CdSe under pressure. Proceedings of the National Academy of Sciences of the United States of America 105(50), pp. 19612-19616. (10.1073/pnas.0805235105)
- Baburin, I. A., Leoni, S. and Seifert, G. 2008. Enumeration of not-yet-synthesized zeolitic zinc imidazolate MOF networks: a topological and DFT approach. Journal of Physical Chemistry B 112(31), pp. 9437-9443. (10.1021/jp801681w)
Articles
- Sheng, Y. et al. 2024. Confinement and synergy effects of supported-confined bimetal catalysts with superior stability and catalytic activity. Journal of Energy Chemistry 99, pp. 93-99. (10.1016/j.jechem.2024.07.022)
- Al Zoubi, W., Leoni, S., Assfour, B., Allaf, A. W., Kang, J. and Ko, Y. G. 2024. Continuous synthesis of metal oxide‐supported high‐entropy alloy nanoparticles with remarkable durability and catalytic activity in the hydrogen reduction reaction. InfoMat (10.1002/inf2.12617)
- Al Zoubi, W., Al Mahmud, A., Hazmatulhaq, F., Thalji, M. R., Leoni, S., Kang, J. and Ko, Y. G. 2024. Origin of the synergistic effects of bimetallic nanoparticles coupled with a metal oxide heterostructure for accelerating catalytic performance. SusMat 4(3), article number: e216. (10.1002/sus2.216)
- Craco, L. and Leoni, S. 2024. Strange metal and coherence-incoherence crossover in pressurized La3Ni2O7. Physical Review B (Condensed Matter and Materials Physics) 109(16), article number: 165116. (10.1103/PhysRevB.109.165116)
- Craco, L. and Leoni, S. 2024. Effect of localization–delocalization transition on thermoelectric properties of Bi2Te2Se topological insulator. APL Energy 2(1), article number: 16102. (10.1063/5.0173308)
- Craco, L. and Leoni, S. 2023. Normal-state correlated electronic structure of the tetragonal TlNi2Se2 superconductor. Physical Review B 108(4), article number: 45140. (10.1103/PhysRevB.108.045140)
- Craco, L. and Leoni, S. 2023. Orbital-selective mixed-valent Mott/metal phase coexistence in NdNiO2 films. Physical Review Materials 7(4), article number: 44802. (10.1103/PhysRevMaterials.7.044802)
- Al Zoubi, W., Assfour, B., Wahab Allaf, A., Leoni, S., Kang, J. and Ko, Y. G. 2023. Experimental and theoretical investigation of high-entropy-alloy/support as a catalyst for reduction reactions.. Journal of Energy Chemistry 81, pp. 132-142. (10.1016/j.jechem.2023.02.042)
- Craco, L., de Arruda, A. S. and Leoni, S. 2022. Emergent normal-state Mottness in the infinite-layer NdNiO 2 superconductor. Physical Review Research 4(4), article number: 43036. (10.1103/PhysRevResearch.4.043036)
- Kaußler, C. et al. 2022. "Dynamical docking" of cyclic dinuclear au(i) bis-n-heterocyclic complexes facilitates their binding to g-quadruplexes. Inorganic Chemistry 61(50), article number: 20405. (10.1021/acs.inorgchem.2c03041)
- Selli, D., Baburin, I. A., Martonák, R. and Leoni, S. 2022. Ge136 type-II clathrate as precursor for the synthesis of metastable germanium polymorphs: a computational study. Physical Review B 106(17), article number: 174102. (10.1103/PhysRevB.106.174102)
- Osypiw, A. et al. 2022. Solution-processed colloidal quantum dots for light emission. Materials Advances 3, pp. 6773-6790. (10.1039/D2MA00375A)
- Rundle, J. and Leoni, S. 2022. Layered tin chalcogenides SnS and SnSe: lattice thermal conductivity benchmarks and thermoelectric figure of merit. Journal of Physical Chemistry C 126(33), pp. 14036–14046. (10.1021/acs.jpcc.2c02401)
- Selli, D., Donadio, D. and Leoni, S. 2022. PbTe/PbSe thermoelectric nanocomposites: the impact of length modulations on lowering thermal conductivity. Journal of Inorganic and General Chemistry 648(15), article number: e202200048. (10.1002/zaac.202200048)
- Flack, T., Jobbins, S. A., Boulfelfel, S. E. and Leoni, S. 2022. Many-particle Li Ion dynamics in LiMPO4 olivine phosphates (M = Mn, Fe). Journal of Physical Chemistry C 126(30), pp. 12339-12347. (10.1021/acs.jpcc.2c02013)
- Ryník, M., Leoni, S. and Martonák, R. 2022. Pressure-induced structural transformation of clathrate Ge136 via ultrafast recrystallization of an amorphous intermediate. Physical Review B 105(13), article number: 134107. (10.1103/PhysRevB.105.134107)
- Craco, L. and Leoni, S. 2022. Orbital selectivity in the normal state of KFe(2)Se(2) superconductor. European Physical Society Letters 136(2), article number: 27002. (10.1209/0295-5075/ac3f16)
- Pimpao, C. et al. 2021. Mechanisms of irreversible aquaporin-10 inhibition by organogold compounds studied by combined biophysical methods and atomistic simulations. Metallomics 13(9), article number: mfab053. (10.1093/mtomcs/mfab053)
- Craco, L., Carara, S. S. and Leoni, S. 2021. Landau-Fermi liquidness and s-wave superconducting properties of pressurized gray phosphorus. The European Physical Journal B 94(5), article number: 115. (10.1140/epjb/s10051-021-00121-y)
- Craco, L. and Leoni, S. 2021. Orbital-selective nature of the 3d electronic structure of the ThFeAsN superconductor. Physical Review B 103(7), article number: 75110. (10.1103/PhysRevB.103.075110)
- Craco, L., Carara, S. S. and Leoni, S. 2021. Interplay of electric field and disorder in Dirac liquid silicene. The European Physical Journal B 94(2), article number: 47. (10.1140/epjb/s10051-021-00055-5)
- Wragg, D., Leoni, S. and Casini, A. 2020. Aquaporin-driven hydrogen peroxide transport: a case of molecular mimicry?. RSC Chemical Biology 1(5), pp. 390-394. (10.1039/D0CB00160K)
- Craco, L. and Leoni, S. 2020. All-t2g electronic orbital reconstruction of monoclinic MoO2 battery material. Applied Sciences 10(17), article number: 5730. (10.3390/app10175730)
- Craco, L. and Leoni, S. 2020. Mott and pseudogap localization in pressurized NbO2. Physical Review B 102(4), article number: 45142. (10.1103/PhysRevB.102.045142)
- Craco, L. and Leoni, S. 2020. Pressure-induced orbital-selective metal from the Mott insulator BaFe2Se3. Physical Review B 101(24), article number: 245133. (10.1103/PhysRevB.101.245133)
- Craco, L. and Leoni, S. 2019. LDA+DMFT approach to electronic structure of sodium metal. Physical Review B 100(11), article number: 115156. (10.1103/PhysRevB.100.115156)
- Craco, L. and Leoni, S. 2019. Theory of two-fluid metallicity in superconducting FeSe at high pressure. Physical Review B 100(12), pp. -., article number: 121101. (10.1103/PhysRevB.100.121101)
- Wragg, D., de Almeida, A., Casini, A. and Leoni, S. 2019. Unveiling the mechanisms of aquaglyceroporin-3 water and glycerol permeation by metadynamics. Chemistry - A European Journal 25(37), pp. 8713-8718. (10.1002/chem.201902121)
- Craco, L., Carara, S. S. and Leoni, S. 2019. Electronic structure of BiFeO3 in the presence of strong electronic correlations. Physical Review B 99(4), pp. -., article number: 45112. (10.1103/PhysRevB.99.045112)
- Fang, H. et al. 2019. Structural tuning and catalysis of tungsten carbides for the regioselective cleavage of C-O bonds. Journal of Catalysis 369, pp. 283-295. (10.1016/j.jcat.2018.11.020)
- Mósca, A. F. et al. 2018. Molecular basis of Aquaporin-7 permeability regulation by pH. Cells 7(11), article number: 207. (10.3390/cells7110207)
- Craco, L. and Leoni, S. 2018. Microscopic description of localization-delocalization transitions in BaFe2S3. Physical Review B 98(19), pp. -., article number: 195107. (10.1103/PhysRevB.98.195107)
- Wragg, D., De Almeida, A., Bonsignore, R., Kühn, F. E., Leoni, S. and Casini, A. 2018. On the mechanism of Gold/NHC compounds binding to DNA G-quadruplexes: combined metadynamics and biophysical methods. Angewandte Chemie International Edition 57(44), pp. 14524-14528. (10.1002/anie.201805727)
- Jobbins, S. A., Boulfelfel, S. E. and Leoni, S. 2018. Metashooting: a novel tool for free energy reconstruction from polymorphic phase transition mechanisms. Faraday Discussions 211, pp. 235-251. (10.1039/C8FD00053K)
- Rocard, L., Wragg, D., Jobbins, S. A., Luciani, L., Leoni, S., Wouters, J. and Bonifazi, D. 2018. Templated chromophore assembly on peptide scaffolds: a structural evolution. Chemistry - A European Journal, pp. -. (10.1002/chem.201803205)
- Craco, L., Freelon, B., Alafailakawi, A. M., Karki, B. and Leoni, S. 2018. Site-selective electronic structure of pure and doped Ca2 O3 Fe3 S2. Physical Review B 98(4), pp. -., article number: 45130. (10.1103/PhysRevB.98.045130)
- Craco, L., Pereira, T. A. d. S., Ferreira, S. R., Carara, S. S. and Leoni, S. 2018. Kondo-semimetal to Fermi-liquid phase crossover in black phosphorus to pressure-induced orbital-nematic gray phosphorus. Physical Review B 98(3), pp. -., article number: 35114. (10.1103/PhysRevB.98.035114)
- Paściak, M., Welberry, T. R., Kulda, J., Leoni, S. and Hlinka, J. 2018. Dynamic displacement disorder of cubic BaTiO3. Physical Review Letters 120(16), pp. -., article number: 167601. (10.1103/PhysRevLett.120.167601)
- Craco, L., Pereira, T. A. d. S. and Leoni, S. 2017. Electronic structure and thermoelectric transport of black phosphorus. Physical Review B 96(7), article number: 75118. (10.1103/PhysRevB.96.075118)
- Craco, L., Laad, M. S. and Leoni, S. 2017. Microscopic description of insulator-metal transition in high-pressure oxygen. Scientific Reports 7, article number: 2632. (10.1038/s41598-017-02730-z)
- De Almeida, A. et al. 2017. The mechanism of aquaporin inhibition by gold compounds elucidated by biophysical and computational methods. Chemical Communications 53(27), pp. 3830-3833. (10.1039/C7CC00318H)
- Craco, L. and Leoni, S. 2017. Selective orbital reconstruction in tetragonal FeS: A density functional dynamical mean-field theory study. Scientific Reports 7, article number: 46439. (10.1038/srep46439)
- Craco, L., Faria, J. L. B. and Leoni, S. 2017. Electronic reconstruction of hexagonal FeS: a view from density functional dynamical mean-field theory. Materials Research Express 4(3), article number: 36303. (10.1088/2053-1591/aa6296)
- Springer, S., Heidenreich, N., Stock, N., van Wüllen, L., Huber, K., Leoni, S. and Wiebcke, M. 2017. The ZIF system zinc(II) 4,5-dichoroimidazolate: theoretical and experimental investigations of the polymorphism and crystallization mechanisms. Zeitschrift für Kristallographie - Crystalline Materials 232(1-3), pp. 77-90. (10.1515/zkri-2016-1968)
- Fang, H., Zheng, J., Luo, X., Du, J., Roldan Martinez, A., Leoni, S. and Yuan, Y. 2017. Product tunable behavior of carbon nanotubes-supported Ni?Fe catalysts for guaiacol hydrodeoxygenation. Applied Catalysis A: General 529, pp. 20-31. (10.1016/j.apcata.2016.10.011)
- Craco, L., Carara, S. S. and Leoni, S. 2016. Band narrowing and Mott localization in isotropically superstrained graphene. Physical Review B 94(16), article number: 165168. (10.1103/PhysRevB.94.165168)
- Springer, S., Baburin, I., Heinemeyer, T., Gerrit Schiffmann, J., van Wullen, L., Leoni, S. and Wiebcke, M. 2016. A zeolitic imidazolate framework with conformational variety: Conformational polymorphs versus frameworks with static conformational disorder. Crystengcomm 18(14), pp. 2477-2489. (10.1039/C6CE00312E)
- Grundy, D. J., Chen, M., Gonzalez, V., Leoni, S., Miller, D. J., Christianson, D. W. and Allemann, R. K. 2016. Mechanism of germacradien-4-ol synthase controlled water capture. Biochemistry 55(14), pp. 2112-2121. (10.1021/acs.biochem.6b00115)
- Selli, D., Boulfelfel, S. E., Schapotschnikow, P., Donadio, D. and Leoni, S. 2016. Hierarchical thermoelectrics: crystal grain boundaries as scalable phonon scatterers. Nanoscale 8(6), pp. 3729-3728. (10.1039/C5NR05279C)
- Freelon, B. et al. 2015. Mott-Kondo insulator behavior in the iron oxychalcogenides. Physical Review B 92(15), article number: 155139. (10.1103/PhysRevB.92.155139)
- Behrens, K. et al. 2015. Microwave-assisted synthesis of defects metal-imidazolate-amide-imidate frameworks and improved CO2 capture. Inorganic Chemistry 54(20), pp. 10073-10080. (10.1021/acs.inorgchem.5b01952)
- Craco, L., Selli, D., Seifert, G. and Leoni, S. 2015. Revealing the hidden correlated electronic structure of strained graphene. Physical Review B 91(20), article number: 205120. (10.1103/PhysRevB.91.205120)
- Craco, L. and Leoni, S. 2015. Magnetoresistance in the spin-orbit kondo state of elemental bismuth. Scientific Reports 5(1), pp. -., article number: 13772. (10.1038/srep13772)
- Craco, L. and Leoni, S. 2014. Effect of band filling in the paramagnetic tetragonal phase of iron chalcogenides. Materials Research Express 1(3), article number: 36001. (10.1088/2053-1591/1/3/036001)
- Boulfelfel, S. E., Selli, D. and Leoni, S. 2014. Novel carbons: habits and oddities. Journal of Inorganic and General Chemistry 640(5), pp. 681-688. (10.1002/zaac.201300652)
- Schweinefuß, M. E., Springer, S., Baburin, I. A., Hikov, T., Huber, K., Leoni, S. and Wiebcke, M. 2014. Zeolitic imidazolate framework-71 nanocrystals and a novel SOD-type polymorph: solution mediated phase transformations, phase selection via coordination modulation and a density functional theory derived energy landscape. Dalton Transactions 43(9), pp. 3528-3536. (10.1039/c3dt52992d)
- Pasciak, M., Welberry, T., Heerdegen, A., Laguta, V., Ostapchuk, T., Leoni, S. and Hlinka, J. 2014. Atomistic modeling of diffuse scattering in cubic PbZrO3. Phase Transitions 88(3), pp. 273-28. (10.1080/01411594.2014.981266)
- Schröder, C. A., Saha, S., Huber, K., Leoni, S. and Wiebcke, M. 2014. Metastable metal imidazolates: development of targeted syntheses by combining experimental and theoretical investigations of the formation mechanisms. Zeitschrift fur Kristallographie Crystalline Materials 229(12), pp. 807-822. (10.1515/zkri-2014-1788)
- Craco, L., Laad, M. S. and Leoni, S. 2014. Orbital-selective mottness in layered iron oxychalcogenides: the case of Na2Fe2OSe2. Journal of Physics: Condensed Matter 26(14), pp. -., article number: 145602. (10.1088/0953-8984/26/14/145602)
- Craco, L., Laad, M. S. and Leoni, S. 2014. Normal-state correlated electronic structure of tetragonal FeSe superconductor. Journal of Physics: Conference Series 487, pp. -., article number: 12017. (10.1088/1742-6596/487/1/012017)
- Schweinefuß, M. E., Baburin, I. A., Schröder, C. A., Näther, C., Leoni, S. and Wiebcke, M. 2014. Indium imidazolate frameworks with differently distorted ReO3-type structures: syntheses, structures, phase transitions, and crystallization studies. Crystal Growth and Design 14(9), pp. 4664-4673. (10.1021/cg5007499)
- Selli, D., Baburin, I. A., Martonák, R. and Leoni, S. 2013. Novel metastable metallic and semiconducting germaniums. Scientific Reports 3, article number: 1466. (10.1038/srep01466)
- Schröder, C. A., Baburin, I. A., van Wüllen, L., Wiebcke, M. and Leoni, S. 2013. Subtle polymorphism of zinc imidazolate frameworks: temperature-dependent ground states in the energy landscape revealed by experiment and theory. Crystengcomm 15(20), pp. 4036-4040. (10.1039/c2ce26045j)
- Baldoni, M., Craco, L., Seifert, G. and Leoni, S. 2013. A two-electron mechanism of lithium insertion into layered α-MoO3: a DFT and DFT+U study. Journal of Materials Chemistry A 1(5), pp. 1778-1784. (10.1039/c2ta00839d)
- Debatin, F. et al. 2012. An isoreticular family of microporous metal-organic frameworks based on zinc and 2-substituted imidazolate-4-amide-5-imidate: syntheses, structures and properties. Chemistry - a European Journal 18(37), pp. 11630-11640. (10.1002/chem.201200889)
- Boulfelfel, S. E., Oganov, A. R. and Leoni, S. 2012. Understanding the nature of 'superhard graphite'. Scientific Reports 2, article number: 471. (10.1038/srep00471)
- Assfour, B., Leoni, S., Seifert, G. and Baburin, I. A. 2011. Packings of carbon nanotubes - new materials for hydrogen storage. Advanced Materials 23(10), pp. 1237-1241. (10.1002/adma.201003669)
- Leoni, S., Ramlau, R., Meier, K., Schmidt, M. and Schwarz, U. 2008. Nanodomain fragmentation and local rearrangements in CdSe under pressure. Proceedings of the National Academy of Sciences of the United States of America 105(50), pp. 19612-19616. (10.1073/pnas.0805235105)
- Baburin, I. A., Leoni, S. and Seifert, G. 2008. Enumeration of not-yet-synthesized zeolitic zinc imidazolate MOF networks: a topological and DFT approach. Journal of Physical Chemistry B 112(31), pp. 9437-9443. (10.1021/jp801681w)
Book sections
- Flack, T., Jobbins, S. A., Boulfelfel, S. E. and Leoni, S. 2024. Many-Particle Na-Ion Dynamics in NaMPO4 Olivine Phosphates (M = Mn, Fe). In: Hanaor, D. A. H. ed. Computational Design of Battery Materials., Vol. 150. Springer, Cham, pp. 137-167., (10.1007/978-3-031-47303-6_5)
- Leoni, S., Boulfelfel, S. E., Baburin, I. A. and Selli, D. 2014. The rules of metastability: detailed transformation mechanisms in chemical elements by means of molecular dynamics techniques. In: Springborg, M. and Joswig, J. eds. Chemical Modelling : Volume 11., Vol. 11. Royal Society of Chemistry, pp. 30.
Conferences
- Wragg, D., Casini, A. and Leoni, S. 2020. Harvesting free energy landscapes in biological systems. Presented at: International Conference on Bio and Nanomaterials, MSC Cruise, Mediterranean Sea, Italy, 28 Sept - 3 Oct 2019 Presented at Piotto, S. et al. eds.Advances in Bionanomaterials II. Lecture Notes in Bioengineering Springer pp. 64-77., (10.1007/978-3-030-47705-9_7)
- Boulfelfel, S. E., Oganov, A. R. and Leoni, S. 2012. Understanding the nature of 'superhard graphite'. Scientific Reports 2, article number: 471. (10.1038/srep00471)
- Assfour, B., Leoni, S., Seifert, G. and Baburin, I. A. 2011. Packings of carbon nanotubes - new materials for hydrogen storage. Advanced Materials 23(10), pp. 1237-1241. (10.1002/adma.201003669)
- Leoni, S., Ramlau, R., Meier, K., Schmidt, M. and Schwarz, U. 2008. Nanodomain fragmentation and local rearrangements in CdSe under pressure. Proceedings of the National Academy of Sciences of the United States of America 105(50), pp. 19612-19616. (10.1073/pnas.0805235105)
- Baburin, I. A., Leoni, S. and Seifert, G. 2008. Enumeration of not-yet-synthesized zeolitic zinc imidazolate MOF networks: a topological and DFT approach. Journal of Physical Chemistry B 112(31), pp. 9437-9443. (10.1021/jp801681w)
Ymchwil
Research Interests
Nucleation in the Solid State
The detailed investigation of structural reconstruction, in pressure or temperature induced phase transitions, is a major challenge in modern material sciences. The combined use of structural modeling approaches and of different advanced numerical tools allows for a detailed understanding of phase nucleation and growth in the solid state. Therein, intermediate reconstruction steps can be elucidated in detail.
Figure 1: Nucleation and growth of a crystalline pattern from a pristine one: CsCl to Rocksalt phase transition in RbCl. Many nuclei are forming, which interact to build the final material. The result of the calculations is a detailed map of solid state reactivity, containing shape of the nuclei, local atomic rearrangements, reaction rates, and which can provide a realistic visualization of the final material (lower left corner), including domains and grain boundaries
Chemical Bond Reconstruction
Bond reconstruction during phase transitions. In phosphorus (black-P to &lcirc;±-As type) reconstruction takes the form of interfacial Peierls-like chains (Fig. 2a), in germanium the hR8 to cI16 reconstruction takes place as SN2 reaction (Fig. 2b), in carbon (graphite to sp3 polymorphs) as a complex pattern of odd-membered ring formation. In every system considered so far, a clear indication of bond nucleation is apparent. In carbon, different mechanisms are responsible for the formation of distinct sp3 polymorphs (Fig. 3c-d). Each mechanism in turn is initiated by different nucleation pattern, promptly suggesting ways of controlling/influencing the formation of either compound.
Figure 2: Covalent network reconstruction of the elements a) phosphorus, b) germanium, c-d) carbon. a) A17-A7 reconstruction of layered phosphorus: formation of an intermediate Peierls-like (red) chain, triggered by single bond formation, interconnecting the layers. b) Reconstruction of the hR8 network into the cI16 network in germanium: formation of two distinct sets of intertwined Ge-Ge linkages (red and blue). The blue ones contain the reactive, SN2-type bond inversion processes; red ones are on the contrary non-reactive. c-d) Formation of sp3 carbons from graphite, under the effect of cold compression. Distinct nucleation pattern lead to different final topologies. In c), rapid bond growth (vertically in figure) anticipates the formation of five-membered rings, followed by seven-membered ring closure. In d) odd rings are formed more sparsely and locally into a pattern that leads to a distinct sp3 carbon. Clearly, nucleation history affects the accessibility of a particular product, as we learn form simulations.
Novel Carbon Materials
Carbon remains a most versatile material. It has the potential of providing clean and very effective solutions in different areas like hydrogen storage, capacitors, optical and electronic devices. The polymorphism of carbon has been the object of many discoveries over the years. Novel forms, ranging from extended (graphene) to finite (nanotubes and fullerenes) have appeared, with outstanding properties. The polymorphism of carbon can be the source of even more interesting properties. Our recent results are along three lines: a) systematic computational approach to carbon polymorphisms, b) novel superhard and transparent sp3 carbon materials, c) carbon nanotubes assemblies with superior hydrogen storage properties. We start from sp2 carbons, graphite and nanotubes to achieve different forms of sp3 carbons on the one hand; on the other hand we address the question of packing nanotubes (CNTs) in space, with a dramatic boost on their properties as hydrogen adsorbers.
Figure 3: a) Four novel carbons were found from metaD runs. All phases are stackings of corrugated graphene layers interconnected by alternating sequences of odd or even rings. Ring topologies influence hardness and optical propertie. b) CNTs matrices display outstanding hydrogen storage properties. At room temperature they can adsorb up to 5.5 wt.% at 100 bar, which closely approaches the Department of Energy (DOE) target value of 6 wt.%. The process is dominated at its early stage by nucleation at strong absorptions sites, followed by hydrogen filling in space.
Metallorganic framework compounds (MOFs)
MOFs are porous molecular scaffoldings able to accommodate guest molecules, and hydrogen in particular. We have developed and expertise in constructing not-yet-synthesized MOFs, and in assessing their capacities as molecular reservoirs. We have started a systematic investigation of promising hydrogen storage candidate materials to meet this challenge. We focus on open framework zeolitic materials like MOFs, COFs and recently ZIFs. MOFs and ZIFs are mechanically versatile and easy to synthesize. On combining topological enumeration, molecular dynamics and structure optimization we are proposing a catalogue with useful hydrogen uptakes. Upon chemical substitution we are able to enhance their specificity for hydrogen, for instance by introducing polarizing centers in the framework (LiB(imid)4, BIFs). In general it is possible to explore a large number of structure candidates, introduce chemical substitution, and evaluate as storage properties in a systematic and efficient way.
Figure 4: The estimation of hydrogen uptake in MOFs, COFs and ZIFs materials can be reliably calculated using Grand canonical Monte Carlo molecular simulations, which indicate LiB(imid)4 structures based on fau, rho, and gme nets as promising candidates for hydrogen storage applications. Their total hydrogen uptake at 77 K amounts to 7.8, 6.9 and 6.9 wt.%, respectively. Note that hydrogen uptake of the fau-based LiB(imid)4 is comparable to that of MOF-177 (~10.0 wt. %), which is a reference material among experimentally characterized compounds.
Battery materials: Mass and charge transport
Two are the principal computational problems in this area: a correct evaluation of mass diffusion/transport, and a reliable ground-state electronic structure (also for resistivity calculations). Our recent work on Li diffusion in an important battery material LiFePO4 represents a step forward in assessing properties and calculating relevant parameters, like diffusion constants, and represents a viable method for accelerating diffusion, which is a typical bottleneck for MD simulations. This extends the possibilities of molecular dynamics to approaching systems where particle diffusion is the dominating physical/chemical event. It allows collecting a number of relevant trajectories on the one had: on the other, details of local oxidation/reduction steps at metal centers can be addressed.
Figure 5: Different aspects of the computation of material properties for cathode materials. a) Diffusion paths of Li within FePO4. In the presence of antisite disorder, besides the main paths (vertical in figure), the [001] direction (horizontal) is also activated. b) The calculation of the correct ground state by means of DFT+ Hubbard U methods is the starting point for the evaluation of resistivity profiles for charged and discharged FePO4/LiFePO4. The presence of peaks in the dielectric function is related to well-defined oxidations states, Fe2+/Fe3+ for instance.
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CH2118 Adnoddau a Deunyddiau Ynni
CH3304 Cemeg Gorfforol Uwch
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Bywgraffiad
Dipl. Chem. ETH (B.Sc.), EidgenÃssische Technische Hochschule (ETH), ZÃ rich (1993), PhD ETH ZÃ rich (1998). Postdoctoral Fellow, ETH ZÃ rich (1999-2000), Max-Planck Society Postdoctoral Scholarship, Max-Planck Institute CPfS, Dresden (2000-2003), Advanced Research Fellow of the Swiss National Foundation (2004-2006), Research group leader & Lecturer, MPI Dresden and Dresden University of Technology (2006-2010), Habilitation, MPI & Department of Chemistry, Dresden (2009), Senior researcher & group leader, Dresden (2010-2013), Distinguished DFG Heisenberg Fellow (2013).